Indoor photovoltaics are promising to enable self‐powered electronic devices for the Internet of Things. Here, reported is a triple‐anion CH3NH3PbI2−xBrClx perovskite film, of which the bandgap is specially designed for indoor light harvesting to achieve a record high efficiency of 36.2% with distinctive high open circuit voltage (Voc) of 1.028 V under standard 1000 lux fluorescent light. The involvement of both bromide and chloride suppresses the trap‐states and nonradiative recombination loss, exhibiting a remarkable ideality factor of 1.097. The introduction of chloride successfully restrains the halide segregation of iodide and bromide, stabilizing the triple‐anion perovskite film. The devices show an excellent long‐term performance, sustaining over 95% of original efficiency under continuous light soaking over 2000 h. These findings show the importance and potential of I/Br/Cl triple‐anion perovskite with tailored bandgap and suppressed trap‐states in stable and efficient indoor light recycling.

We review two types of inorganic nanomaterials-metal chalcogenide quantum dots (QDs) and lead halide perovskites-that serve as prospective light harvesters in hybrid mesoscopic solar cells. Metal chalcogenide QDs are introduced in three parts: chalcogenides of cadmium (CdS, CdSe and CdTe), chalcogenides of lead (PbS and PbSe) and chalcogenides of antimony (Sb 2 S 3 and Sb 2 Se 3). The devices made using these chalcogenide QDs in a liquid-type electrolyte showed the best cell efficiencies, ranging from 3 to 6%. For solid-state QD-sensitized solar cells (QDSCs), the device performances were generally poor; only devices made of Sb 2 S 3 and PbS QDs attained cell efficiencies approaching B7%. In contrast, nanocrystalline lead halide perovskites have emerged since 2009 as potential photosensitizers in liquid-type sensitized TiO 2 solar cells. In 2012, the efficiencies of the all-solid-state perovskite solar cells were enhanced to 9.7 and 10.9% using anodes of TiO 2 and Al 2 O 3 films, respectively, with 2,2 0 ,7,7 0-tetrakis-(N,N-dip -methoxyphenylamine)9,9 0-spirobifluorene (spiro-OMeTAD) as a holetransporting material. In 2013, the performance of a TiO 2 solar cell sensitized with lead iodide perovskite (CH 3 NH 3 PbI 3) was optimized further to attain an overall power conversion efficiency g ¼ 15%, which is a new milestone for solar cells of this type having a device structure similar to that of a dye-sensitized solar cell.

Reduced graphene oxides (rGO) are synthesized via reduction of GO with reducing agents as a hole‐extraction layer for high‐performance inverted planar heterojunction perovskite solar cells. The best efficiencies of power conversion (PCE) of these rGO cells exceed 16%, much greater than those made of GO and poly(3,4‐ethenedioxythiophene):poly(styrenesulfonate) films. A flexible rGO device shows PCE 13.8% and maintains 70% of its initial performance over 150 bending cycles. It is found that the hole‐extraction period is much smaller for the GO/methylammonium lead‐iodide perovskite (PSK) film than for the other rGO/PSK films, which contradicts their device performances. Photoluminescence and transient photoelectric decays are measured and control experiments are performed to prove that the reduction of the oxygen‐containing groups in GO significantly decreases the ability of hole extraction from PSK to rGO and also retards the charge recombination at the rGO/PSK interface. When the hole injection from PSK to GO occurs rapidly, hole propagation from GO to the indium‐doped tin oxide (ITO) substrate becomes a bottleneck to overcome, which leads to a rapid charge recombination that decreases the performance of the GO device relative to the rGO device.

The excitonic relaxation dynamics of perovskite adsorbed on mesoporous thin films of Al2O3 and NiO upon excitation at 450 nm were investigated with femtosecond optical gating of photoluminescence (PL) via up-conversion. The temporal profiles of emission observed in spectral region 670-810 nm were described satisfactorily with a composite consecutive kinetic model and three transient components representing one hot and two cold excitonic relaxations. All observed relaxation dynamics depend on the emission wavelength, showing a systematic time-amplitude correlation for all three components. When the NiO film was employed, we observed an extent of relaxation proceeding through the non-emissive surface state larger than through the direct electronic relaxation channel, which quenches the PL intensity more effectively than on the Al2O3 film. We conclude that perovskite is an effective hole carrier in a p-type electrode for NiO-based perovskite solar cells showing great performance.

The hybrid perovskite/graphene oxide composite layer increased the interfacial contact between the donor and acceptor of holes to balance the charge mobility and improved the photovoltaic performance with excellent reproducibility and stability.

The excitonic relaxation dynamics of perovskite adsorbed on mesoporous thin films of Al 2 O 3 and NiO upon excitation at 450 nm were investigated with femtosecond optical gating of photoluminescence (PL) via up-conversion. The temporal profiles of emission observed in spectral region 670-810 nm were described satisfactorily with a composite consecutive kinetic model and three transient components representing one hot and two cold excitonic relaxations. All observed relaxation dynamics depend on the emission wavelength, showing a systematic time-amplitude correlation for all three components. When the NiO film was employed, we observed an extent of relaxation proceeding through the nonemissive surface state larger than through the direct electronic relaxation channel, which quenches the PL intensity more effectively than on the Al 2 O 3 film. We conclude that perovskite is an effective hole carrier in a p-type electrode for NiO-based perovskite solar cells showing great performance.

The control of the thickness and porosity of a mesoporous TiO2 layer is important to improve the photovoltaic performance of perovskite solar cells. We produced organized mesoporous TiO2 (om-TiO2) layers using a low-cost amphiphilic graft copolymer, poly­(vinyl chloride)-graft-poly­(oxyethylene methacrylate) (PVC-g-POEM), as a sacrificial template. This simple but effective synthetic approach generates highly mesoporous and well-organized TiO2 nanostructures with interconnected and size-tunable features. Specifically, the average pore size increased with the amount of hydrophobic PVC main chain in the graft copolymer, which acted as the pore forming agent. Perovskite layers were prepared on top of an om-TiO2 layer according to a two-step sequential deposition: after coating the PbI2 solution in dimethylformamide (DMF) on an om-TiO2 substrate, the substrate was prewetted in isopropyl alcohol (IPA) solvent before immersing into a CH3NH3I/IPA solution. This prewetting treatment not only improves the yields of conversion from PbI2 to CH3NH3PbI3, but also increases the size of perovskite crystals with cuboid morphology. On varying the pore size and the film thickness of the om-TiO2 layer, the device performance attained 11.9% of power conversion efficiency (PCE) at pore size 70 nm and film thickness 300 nm. We measured extracted charge densities and decays of transient photovoltage to understand the kinetics of charge recombination in relation to the corresponding device performance.

Solar cells based on organometal-halide perovskites such as CH3NH3PbI3 have emerged as a promising next-generation photovoltaic system, but the underlying photophysics and photochemistry remain to be established because of the limited availability of methods to implement the simultaneous and direct measurement of various charge carriers and ions that play a crucial role in the operating device. We used nanosecond time-resolved infrared (IR) spectroscopy to investigate, with high molecular specificity, distinct transient species that are formed in perovskite solar cells after photoexcitation. In CH3NH3PbI3 planar-heterojuction solar cells, we simultaneously observed infrared spectral signatures that are associated with an intraband transition of conduction-band electrons, Fano resonance, and the spiro-OMeTAD cation having an exceptionally short lifetime of 1.0 μs (at ∼1485 cm(-1)). The present results show that the time-resolved IR method offers a unique capability to elucidate these important transients in perovskite solar cells and their dynamic interplay in a comprehensive manner.